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J Chem Phys. 2004 Oct 22;121(16):7932-45.

Why hyperpolarizabilities fall short of the fundamental quantum limits.

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  • 1Department of Physics, Washington State University, Pullman, WA 99164-2814, USA.

Erratum in

  • J Chem Phys. 2006 Aug 21;125(7):079905.


Quantum sum rules impose limits on the hyperpolarizability, beta. A survey of the largest second-order molecular susceptibilities finds what appears to be a universal gap between the experimental results and the fundamental limits. In this work, we use theory, linear spectroscopy, Raman spectroscopy, and measured values of beta (using hyper-Rayleigh scattering and Stark Spectroscopy) to show that this gap is due to an unfavorable arrangement of excited state energies. The question of whether this result is a universal property of a quantum system or a matter of present paradigms for making molecules is discussed.

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